Super-resolution lifetime imaging of single molecules surrounding gold bowtie nanoparticles
Authors
Hallenbeck, Zachary
ORCID
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Other Contributors
N'Gom, Moussa
Ullal, Chaitanya
Wang, G.-C. (Gwo-Ching), 1946-
Wertz, Esther A.
Ullal, Chaitanya
Wang, G.-C. (Gwo-Ching), 1946-
Wertz, Esther A.
Issue Date
2022-05
Keywords
Physics
Degree
PhD
Terms of Use
Attribution-NonCommercial-NoDerivs 3.0 United States
This electronic version is a licensed copy owned by Rensselaer Polytechnic Institute (RPI), Troy, NY. Copyright of original work retained by author.
This electronic version is a licensed copy owned by Rensselaer Polytechnic Institute (RPI), Troy, NY. Copyright of original work retained by author.
Full Citation
Abstract
Interactions between light and matter serve as the basis of many of the technologies weuse, whether it be photon absorption, emission, or other transfers of energy. The quality of these
devices is thus inherently limited by the optical properties of their constituents, which are regularly
quite lacking in efficiency. Plasmonic nanoparticles serve as a highly versatile and tunable
platform for the enhancement of such optical properties when one of these optical transitions
occurs in their near-field. However, the near-field nature of these effects has made thorough study
and understanding of these mechanisms difficult. Particularly, a study of molecular decay rate
enhancement in resonant plasmonic environments on this length scale has only recently been
performed, and with limitations on efficiency and resolution. In this dissertation, I describe a new
technique that combines super-resolution microscopy with fluorescence lifetime imaging
microscopy (FLIM) to study single-molecule decay rate enhancement in a single-measurement,
with spatial resolution on the order of 10 nm. Additionally, in the same measurement, we verify
the validity of this technique using autocorrelation to confirm that our data indeed originates from
individual molecules, avoiding ensemble averaging. This thesis provides further insight into the
various mechanisms of plasmon-enhanced emission, decoupled from absorption enhancement,
providing a platform for further study of emission mislocalization and the position-dependent
prominence of different decay pathways.
Description
May 2022
School of Science
School of Science
Department
Dept. of Physics, Applied Physics, and Astronomy
Publisher
Rensselaer Polytechnic Institute, Troy, NY
Relationships
Rensselaer Theses and Dissertations Online Collection
Access
CC BY-NC-ND. Users may download and share copies with attribution in accordance with a Creative Commons
Attribution-Noncommercial-No Derivative Works 3.0 license. No commercial use or derivatives
are permitted without the explicit approval of the author.